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- ItemConfined crystals of the smallest phase-change material(Washington, DC : American Chemical Society, 2013) Giusca, C.E.; Stolojan, V.; Sloan, J.; Börrnert, F.; Shiozawa, H.; Sader, K.; Rümmeli, M.H.; Büchner, B.; Silva, S.R.P.The demand for high-density memory in tandem with limitations imposed by the minimum feature size of current storage devices has created a need for new materials that can store information in smaller volumes than currently possible. Successfully employed in commercial optical data storage products, phase-change materials, that can reversibly and rapidly change from an amorphous phase to a crystalline phase when subject to heating or cooling have been identified for the development of the next generation electronic memories. There are limitations to the miniaturization of these devices due to current synthesis and theoretical considerations that place a lower limit of 2 nm on the minimum bit size, below which the material does not transform in the structural phase. We show here that by using carbon nanotubes of less than 2 nm diameter as templates phase-change nanowires confined to their smallest conceivable scale are obtained. Contrary to previous experimental evidence and theoretical expectations, the nanowires are found to crystallize at this scale and display amorphous-to-crystalline phase changes, fulfilling an important prerequisite of a memory element. We show evidence for the smallest phase-change material, extending thus the size limit to explore phase-change memory devices at extreme scales.
- ItemNesting-driven multipolar order in CeB6 from photoemission tomography(London : Nature Publishing Group, 2016) Koitzsch, A.; Heming, N.; Knupfer, M.; Büchner, B.; Portnichenko, P.Y.; Dukhnenko, A.V.; Shitsevalova, N.Y.; Filipov, V.B.; Lev, L.L.Some heavy fermion materials show so-called hidden-order phases which are invisible to many characterization techniques and whose microscopic origin remained controversial for decades. Among such hidden-order compounds, CeB6 is of model character due to its simple electronic configuration and crystal structure. Apart from more conventional antiferromagnetism, it shows an elusive phase at low temperatures, which is commonly associated with multipolar order. Here we show that this phase roots in a Fermi surface instability. This conclusion is based on a full 3D tomographic sampling of the electronic structure by angle-resolved photoemission and comparison with inelastic neutron scattering data. The hidden order is mediated by itinerant electrons. Our measurements will serve as a paradigm for the investigation of hidden-order phases in f-electron systems, but also generally for situations where the itinerant electrons drive orbital or spin order.
- ItemHigh-field ESR studies of the quantum spin magnet CaCu2O 3(Milton Park : Taylor & Francis, 2006) Goiran, M.; Costes, M.; Broto, J.M.; Chou, F.C.; Klingeler, R.; Arushanov, E.; Drechsler, S.-L.; Büchner, B.; Kataev, V.We report an electron spin resonance (ESR) study of the s = 1/2 Heisenberg pseudo-ladder magnet CaCu2O3 in pulsed magnetic fields up to 40 T. At sub-terahertz frequencies we observe an ESR signal originating from a small amount of uncompensated spins residing presumably at the imperfections of the strongly antiferromagnetically correlated host spin lattice. The data give evidence that these few per cent of 'extra' spin states are coupled strongly to the bulk spins and are involved in the antiferromagnetic (AF) ordering at TN = 25 K. By mapping the frequency/resonance field diagram we have determined a small gap for magnetic excitations below TN of the order of ~0.3–0.8 meV. Such a small value of the gap explains the occurrence of the spin-flop transition in CaCu2O3 at weak magnetic fields μ0Hsf ~ 3 T. Qualitative changes of the ESR response with the increasing field strength give indications that strong magnetic fields reduce the AF correlations and may even suppress the long-range magnetic order in CaCu2O3. ESR data support scenarios with a significant role of the 'extra' spin states for the properties of low-dimensional quantum magnets.
- ItemOptical study of orbital excitations in transition-metal oxides(Milton Park : Taylor & Francis, 2005) Rückamp, R.; Benckiser, E.; Haverkort, M.W.; Roth, H.; Lorenz, T.; Freimuth, A.; Jongen, L.; Möller, A.; Meyer, G.; Reutler, P.; Büchner, B.; Revcolevschi, A.; Cheong, S.-W.; Sekar, C.; Krabbes, G.; Grüninger, M.The orbital excitations of a series of transition-metal compounds are studied by means of optical spectroscopy. Our aim was to identify signatures of collective orbital excitations by comparison with experimental and theoretical results for predominantly local crystal-field excitations. To this end, we have studied TiOCl, RTiO3 (R = La, Sm and Y), LaMnO3, Y2BaNiO5, CaCu2O3 and K4Cu4OCl10, ranging from early to late transition-metal ions, from t2g to eg systems, and including systems in which the exchange coupling is predominantly three-dimensional, one-dimensional or zero-dimensional. With the exception of LaMnO3, we find orbital excitations in all compounds. We discuss the competition between orbital fluctuations (for dominant exchange coupling) and crystal-field splitting (for dominant coupling to the lattice). Comparison of our experimental results with configuration-interaction cluster calculations in general yields good agreement, demonstrating that the coupling to the lattice is important for a quantitative description of the orbital excitations in these compounds. However, detailed theoretical predictions for the contribution of collective orbital modes to the optical conductivity (e.g. the line shape or the polarization dependence) are required to decide on a possible contribution of orbital fluctuations at low energies, in particular, in case of the orbital excitations at ≈0.25 eV in RTiO3. Further calculations are called for which take into account the exchange interactions between the orbitals and the coupling to the lattice on an equal footing.
- ItemOrbital and spin effects for the upper critical field in As-deficient disordered Fe pnictide superconductors(Milton Park : Taylor & Francis, 2009) Fuchs, G.; Drechsler, S.-L.; Kozlova, N.; Bartkowiak, M.; Hamann-Borrero, J.E.; Behr, G.; Nenkov, K.; Klauss, H.-H.; Maeter, H.; Amato, A.; Luetkens, H.; Kwadrin, A.; Khasanov, R.; Freudenberger, J.; Köhler, A.; Knupfer, M.; Arushanov, E.; Rosner, H.; Büchner, B.; Schultz, L.We report upper critical field Bc2(T) data for LaO0.9F0.1FeAs1- δ in a wide temperature and field range up to 60 T. The large slope of Bc2≈- 5.4 to -6.6 T K-1 near an improved Tc≈28.5 K of the in-plane Bc2(T) contrasts with a flattening starting near 23 K above 30 T we regard as the onset of Pauli-limited behaviour (PLB) with Bc2(0)≈63–68 T. We interpret a similar hitherto unexplained flattening of the Bc2(T) curves reported for at least three other disordered closely related systems, Co-doped BaFe2As2, (Ba,K) Fe2As2 and NdO0.7F0.3FeAs (all single crystals), for applied fields H∥(a,b), also as a manifestation of PLB. Their Maki parameters have been estimated by analysing their Bc2(T) data within the Werthamer–Helfand–Hohenberg approach. The pronounced PLB of (Ba, K)Fe2As2 single crystals obtained from an Sn flux is attributed also to a significant As deficiency detected by wavelength dispersive x-ray spectroscopy as reported by Ni et al (2008 Phys. Rev. B 78 014507). Consequences of our results are discussed in terms of disorder effects within conventional superconductivity (CSC) and unconventional superconductivity (USC). USC scenarios with nodes on individual Fermi surface sheets (FSS), e.g. p- and d-wave SC, can be discarded for our samples. The increase of dBc2/dT|Tc by sizeable disorder provides evidence for an important intraband (intra-FSS) contribution to the orbital upper critical field. We suggest that it can be ascribed either to an impurity-driven transition from s± USC to CSC of an extended s++-wave state or to a stabilized s±-state provided As-vacancies cause predominantly strong intraband scattering in the unitary limit. We compare our results with Bc2 data from the literature, which often show no PLB for fields below 60–70 T probed so far. A novel disorder-related scenario of a complex interplay of SC with two different competing magnetic instabilities is suggested.
- ItemSurface and bulk electronic structure of the unconventional superconductor Sr2RuO4: Unusual splitting of the β band(Milton Park : Taylor & Francis, 2012) Zabolotnyy, V.B.; Carleschi, E.; Kim, T.K.; Kordyuk, A.A.; Trinckauf, J.; Geck, J.; Evtushinsky, D.; Doyle, B.P.; Fittipaldi, R.; Cuoco, M.; Vecchione, A.; Büchner, B.; Borisenko, S.V.We present an angle-resolved photoemission study of the surface and bulk electronic structure of the single layer ruthenate Sr2RuO4. As the early studies by photoemission and scanning tunneling microscopy were confronted with a problem of surface reconstruction, surface ageing was previously proposed as a possible remedy to access the bulk states. Here, we suggest an alternative way by demonstrating that, in the case of Sr2RuO4, circularly polarized light can be used to disentangle the signals from the bulk and surface layers, thus opening the possibility to investigate many-body interactions both in bulk and surface bands. The proposed procedure results in improved momentum resolution, which enabled us to detect an unexpected splitting of the surface β band. We discuss the origin of the splitting of the β band and the possible connection with the Rashba effect at the surface.
- ItemFermi surface nesting in several transition metal dichalcogenides(Milton Park : Taylor & Francis, 2008) Inosov, D.S.; Zabolotnyy, V.B.; Evtushinsky, D.V.; Kordyuk, A.A.; Büchner, B.; Follath, R.; Berger, H.; Borisenko, S.V.By means of high-resolution angle-resolved photoelectron spectroscopy (ARPES), we have studied the fermiology of 2H transition metal dichalcogenide polytypes TaSe2, NbSe2 and Cu0.2NbS 2. The tight-binding model of the electronic structure, extracted from ARPES spectra for all three compounds, was used to calculate the Lindhard function (bare spin susceptibility), which reflects the propensity to charge density wave (CDW) instabilities observed in TaSe2 and NbSe 2. We show that though the Fermi surfaces of all three compounds possess an incommensurate nesting vector in the close vicinity of the CDW wave vector, the nesting and ordering wave vectors do not exactly coincide, and there is no direct relationship between the magnitude of the susceptibility at the nesting vector and the CDW transition temperature. The nesting vector persists across the incommensurate CDW transition in TaSe2 as a function of temperature despite the observable variations of the Fermi surface geometry in this temperature range. In Cu0.2NbS2, the nesting vector is present despite different doping levels, which leads us to expect a possible enhancement of the CDW instability with Cu intercalation in the Cu xNbS2 family of materials.
- ItemElectronic depth profiles with atomic layer resolution from resonant soft x-ray reflectivity(Milton Park : Taylor & Francis, 2015) Zwiebler, M.; Hamann-Borrero, J.E.; Vafaee, M.; Komissinskiy, P.; Macke, S.; Sutarto, R.; He, F.; Büchner, B.; Sawatzky, G.A.; Alff, L.; Geck, J.The analysis of x-ray reflectivity data from artificial heterostructures usually relies on the homogeneity of optical properties of the constituent materials. However, when the x-ray energy is tuned to the absorption edge of a particular resonant site, this assumption may no longer be appropriate. For samples realizing lattice planes with and without resonant sites, the corresponding regions containing the sites at resonance will have optical properties very different from regions without those sites. In this situation, models assuming homogeneous optical properties throughout the material can fail to describe the reflectivity adequately. As we show here, resonant soft x-ray reflectivity is sensitive to these variations, even though the wavelength is typically large as compared to the atomic distances over which the optical properties vary. We have therefore developed a scheme for analyzing resonant soft x-ray reflectivity data, which takes the atomic structure of a material into account by 'slicing' it into atomic planes with characteristic optical properties. Using LaSrMnO4 as an example, we discuss both the theoretical and experimental implications of this approach. Our analysis not only allows to determine important structural information such as interface terminations and stacking of atomic layers, but also enables to extract depth-resolved spectroscopic information with atomic resolution, thus enhancing the capability of the technique to study emergent phenomena at surfaces and interfaces.
- ItemAbsorption and photoemission spectroscopy of rare-earth oxypnictides(Milton Park : Taylor & Francis, 2009) Kroll, T.; Roth, F.; Koitzsch, A.; Kraus, R.; Batchelor, D.R.; Werner, J.; Behr, G.; Büchner, B.; Knupfer, M.The electronic structure of various rare-earth oxypnictides has been investigated by performing Fe L2, 3 x-ray absorption spectroscopy, and Fe 2p and valence band x-ray photoemission spectroscopy. As representative samples the non-superconducting parent compounds LnFeAsO (Ln=La, Ce, Sm and Gd) have been chosen and measured at 25 and 300 K, i.e. below and above the structural and magnetic phase transition at ~150 K. We find no significant change of the electronic structure of the FeAs layers when switching between the different rare-earth ions or when varying the temperature below and above the transition temperatures. Using a simple two-configuration model, we find qualitative agreement with the Fe 2p3/2 core-level spectrum, which allows for a qualitative explanation of the experimental spectral shapes.
- ItemOrbital order induced ferromagnetic insulating properties(Milton Park : Taylor & Francis, 2004) Geck, J.; Wochner, P.; Kiele, S.; Klingeler, R.; Revcolevschi, A.; v. Zimmermann, M.; Büchner, B.; Reutler, P.At temperatures below the metal-insulator transition of La 1-xSrxMnO3 with 0.1 < x < 0.15, a peculiar ferromagnetic and insulating phase is observed which has been intensively discussed over the last few years. We present a detailed investigation of this phase by means of resonant and high energy x-ray scattering along with measurements of the electrical resistivity, thermal expansion, magnetization, and specific heat. Interestingly, the data show that the metal-insulator transition of lightly doped manganites is accompanied by an orbital rearrangement. The microscopic information provided by the x-ray scattering studies together with the analysis of the macroscopic properties implies that the orbital reordering maximizes the gain of double exchange energy and, at the same time, induces an insulating behaviour. The relevance of the double-exchange mechanism for the stabilization of the ferromagnetic insulating phase is further substantiated by studies of (La1-yPr y)7/8Sr1/8MnO3: with increasing praseodymium content, the metal-insulator transition is dramatically suppressed which can naturally be explained by a reduction of the band width upon praseodymium doping.